Circumventing bottlenecks in H2O2 photosynthesis over carbon nitride with iodine redox chemistry and electric field effects

Chang-Wei Bai, Lian-Lian Liu, Jie-Jie Chen, Fei Chen (), Zhi-Quan Zhang, Yi-Jiao Sun, Xin-Jia Chen, Qi Yang and Han-Qing Yu ()
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Chang-Wei Bai: Chongqing University
Lian-Lian Liu: University of Science and Technology of China
Jie-Jie Chen: University of Science and Technology of China
Fei Chen: Chongqing University
Zhi-Quan Zhang: Chongqing University
Yi-Jiao Sun: Chongqing University
Xin-Jia Chen: Chongqing University
Qi Yang: Hunan University
Han-Qing Yu: University of Science and Technology of China

Nature Communications, 2024, vol. 15, issue 1, 1-16

Abstract: Abstract Artificial photosynthesis using carbon nitride (g-C3N4) holds a great promise for sustainable and cost-effective H2O2 production, but the high carrier recombination rate impedes its efficiency. To tackle this challenge, we propose an innovative method involving multispecies iodine mediators (I−/I3−) intercalation through a pre-photo-oxidation process using potassium iodide (suspected deteriorated “KI”) within the g-C3N4 framework. Moreover, we introduce an external electric field by incorporating cationic methyl viologen ions to establish an auxiliary electron transfer channel. Such a unique design drastically improves the separation of photo-generated carriers, achieving an impressive H2O2 production rate of 46.40 mmol g−1 h−1 under visible light irradiation, surpassing the most visible-light H2O2-producing systems. Combining various advanced characterization techniques elucidates the inner photocatalytic mechanism, and the application potential of this photocatalytic system is validated with various simulation scenarios. This work presents a significative strategy for preparing and applying highly efficient g-C3N4-based catalysts in photochemical H2O2 production.

Date: 2024
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DOI: 10.1038/s41467-024-49046-x

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